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Chinese Chemical Letters 2025年第2期36卷 360-365页

作者： Yi Zhou Wei Zhang Rong Fu Jiaxin Dong Yuxuan Liu Zihang Song Han Han Kang Cai College of chemistry Nankai University department of chemistry Northwestern University department of chemistry The University of Hong Kong

Chiral coordination molecular cages/capsules with discrete nanoconfined chiral cavities demonstrate significant potential applications across various fields. In this study, we utilized Tr?ger's base as the building block to design and synthesize two pairs of enantiopure ligands. These ligands were then self-assembled with Pd(II) ions through chiral self-sorting coordination, resulting in the formation of two pairs of homochiral M2L4-type coordination molecular capsules. Notably, due to differences in the substitution positions on the Tr?ger's base, these two pairs of enantiomeric coordination molecular capsules exhibited distinct levels of cavity closures, cavity sizes, and host-guest recognition properties. This research offers valuable insights into the construction of novel chiral molecular capsules and the regulation of confined cavities.

关键词： Chirality Host-guest recognition Metal-organic capsule Self-sorting Tröger's base

Neuromodulation with chemicals:Opportunities and challenges

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Fundamental Research 2025年第1期5卷 55-62页

作者： Yifei Pan Cong Pan Lanqun Mao Ping Yu Key Laboratory of analytical chemistry for Living Biosystems Institute of chemistry Chinese Academy of SciencesBeijing 100190China College of chemistry Beijing Normal UniversityBeijing 100875China

Chemicals play a crucial role in neurophysiological and neuropathological *** regulating the concentration of specific chemicals,receptors on the neuron cell membrane can be modulated to activate or inhibit,thereby influencing specific ion channels and facilitating *** review introduces several chemical modulation techniques,such as microinjection,electrode/nanoparticle-based chemical delivery methods,in situ electrochemical synthesis and *** these techniques show promise in expanding the application of chemical neuromodulation,they currently exhibit different degrees of shortcomings and room for *** review summarizes the opportunities and challenges for chemical neuromodulation methods and provide an outlook for their prospects in the future.

关键词： Neuromodulation Chemical delivery Brain chemistry Neurochemistry In vivo

Revealing the difference of Stark tuning rate between interface and bulk by surface-enhanced infrared absorption spectroscopy

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Chinese Chemical Letters 2025年第2期36卷 461-464页

作者： Manyu Zhu Fei Liang Lie Wu Zihao Li Chen Wang Shule Liu Xiue Jiang State Key Laboratory of Electroanalytical chemistry Changchun Institute of Applied ChemistryChinese Academy of Sciences School of Applied chemistry and Engineering University of Science and Technology of China School of Materials Science and Engineering Sun Yat-sen University Research Center for analytical Science College of ChemistryNankai University

Revealing the factors that affect the vibrational frequency of Stark probe at interface is a pre-requirement for evaluating the absolute interfacial electric *** using surface-enhanced infrared absorption(SEIRA) spectroscopy,attenuated total reflection (ATR) spectroscopy and molecular dynamics (MD),we reveal the assembled C≡N at gold nanofilm exhibits a reduced Stark tuning rate (STR) referring to the vibrational frequency shift in response to electric field comparing with the bulk which was regulated by the electron transfer between S and *** findings lead to a deeper understanding of the vibrational Stark effect at the interface and provide guidance for improving the interface electric field theory.

关键词： Attenuated total reflection spectroscopy Cyano group Stark tuning rate Surface-enhanced infrared spectroscopy Vibrational stark effect

Self-sustainable Catalytic Nucleic Acid Circuit Powered Hybrid CRISPR-Cas Systems for Point-of-Care Diagnosis of Circadian Clock Gene from Cell Lysates

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Journal of Analysis and Testing 2025年第01期 1-11页

作者： Zhiyuan Feng Ran Liu Enming Yang Rui Lian Jingjing Zhang State Key Laboratory of analytical chemistry for Life Science School of Chemistry and Chemical Engineering Chemistry and Biomedicine Innovation Center (ChemBIC)Nanjing University

The CRISPR-Cas13 systems have opened a new avenue for RNA detection due to their exceptional programmable collateral activity against ssRNA. However, most high-performance Cas13-based RNA sensors still suffer from some drawbacks because of the tradeoffs between readout device complexity and analytical sensitivity, which can limit their viability at the point-of-care(POC). To overcome these shortcomings, we herein report a novel target-responsive POC platform for translating RNA detection into a glucose test. Specifically, this platform combines the advantages of three techniques: a hybrid Cas13a/Cas12a system for both RNA recognition with single-base resolution and cascade enzymatic amplification, a self-sustainable catalytic nucleic acid circuit(SCC) with embedded uracil-base and poly-T bulges for Cas13a-and Cas12amediated collateral cleavage, respectively, and a portable glucose meter(PGM) for simple signal readout. The incorporation of an engineered ssDNA–invertase conjugate in SCC led to RNA-to-glucose signal transduction through the hydrolysis of sucrose to glucose. By targeting a 20-nt conserved region of BMAL1 mRNA(mBMAL1), a key circadian clock gene, we demonstrate that SCC can serve as an excellent CRISPR reporter, enabling the direct detection of unamplified mBMAL1 as low as 0.864 fM concurrently with good discrimination ability for single-base mismatch. More importantly, this integrated platform was successfully applied for POC diagnosis of mBMAL1 from different cell lysates, with results that strongly correlate with RT-PCR. Given its wide adaptability, we anticipate that such a CRISPR-SCC system can be easily modified to quantify other RNA biomarkers associated with circadian rhythm.

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The transformation of nor-seco-cucurbit[10]uril to cucurbit[5]uril and cucurbit[8]uril controlled by its own concentration

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Chinese Chemical Letters 2025年第2期36卷 373-377页

作者： Shaojie Deng Peihua Ma Qinghong Bai Xin Xiao Key Laboratory of Macrocyclic and Supramolecular chemistry of Guizhou Province Department of Chemistry Guizhou University

Nor-seco-cucurbit[10]uril(ns-CB[10]) is a kinetic product with unique structure. The single bridged methylene in its structure makes the molecular cavity of ns-CB[10] more deformable when compared to ordinary cucurbit[n]uril, reducing its structural stability. Repeated experiments showed that ns-CB[10] gradually cracks in an acidic solution and changes the specificity of cucurbit[5]uril(CB[5]) and cucurbit[8]uril(CB[8]) under more robust acidic solutions and when heated. A series of experiments were designed to study the transformation behavior of ns-CB[10]. It was found that the concentration of ns-CB[10] was correlated with the content distribution of CB[5] and CB[8]. This study explores the influencing factors and mechanisms of the transformation of ns-CB[10] to CB[5] and CB[8]. The results are of great significance for the application of ns-CB[10], understanding the formation mechanism of cucurbit[n]urils. Furthermore,it provides a new pathway for synthesizing new cucurbit[n]urils.

关键词： Concentration control Cracking Mechanism Nor-seco-cucurbituril Transformation

Piling up multidecker pyrgos[n]cages as antibacterial materials

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Science China Materials 2025年第1期68卷 314-316页

作者： Miguel A.Liuzzi-Vaamonde Jackson B.Lancaster Samantha A.Mason Yuanning Feng department of chemistry and Biochemistry The University of OklahomaOklahoma 73019United States

The development of antibiotics is regarded as one of the most significant scientific advances in modern medicine. Before the commercialization of antibiotics, infectious diseases were catastrophic throughout history [1]. Penicillin was used to treat serious infections in the 1940s, but unfortunately, with the introduction of antibiotics came the emergence of antibiotic resistance [2,3]. Evolved and adapted methicillin-resistant Staphylococcus aureus (MRSA) strains are presently impacting community and healthcare systems across the globe [4].

关键词： diseases adapted antibiotics

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Enantioselective copper-catalyzed dearomative borylative cyclization of indoles and mechanistic insights

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Science China chemistry 2025年第2期68卷 670-678页

作者： Yanfei Li Xuetao Li Zheng Zhang Yiliang Zhang Xiuping Yuan Jianjun Yin Simin Wang Wei Guan Qian Zhang Tao Xiong Jilin Province Key Laboratory of Organic Functional Molecular Design&Synthesis Department of ChemistryNortheast Normal UniversityChangchun 130024China Institute of Functional Material chemistry Department of ChemistryNortheast Normal UniversityChangchun 130024China State Key Laboratory of Organometallic chemistry Shanghai Institute of Organic ChemistryChinese Academy of SciencesShanghai 200032China School of chemistry and Chemical Engineering Harbin Normal UniversityHarbin 150025China

Alicyclic nitrogen heterocycles,such as enantioenriched polycyclic fused[1,2-a]indoline derivatives,are widespread in natural products,agrochemicals and pharmaceutical *** methods predominantly rely on the recent emerging Heck-type catalytic asymmetric dearomatization(CADA)protocol,wherein noble palladium catalysts commonly necessitate the form arylPd species-triggered these *** contrast,a more sustainable base metal catalysis paradigm through alkyl metal species disrupting the aromaticity,that is,the utilization of challenging asymmetric Csp3–Csp3 bond formation entry to such important chiral densely functionalized polycyclic molecular scaffolds,remains an elusive ***,we report the first copper-catalyzed dearomative borylative cyclization of indoles under mild reaction conditions,affording an array of valuable Bpin-containing pyrrolo-fused[1,2-a]indolines bearing four consecutive stereogenic centers with excellent enantioand *** synthetic potential was documented via an array of useful *** functional theory(DFT)calculation studies elucidated the origin of the chemo-,regio-,enantio-and diastereoselectivities of this conversion.

关键词： copper catalysis dearomatization borylative cyclization indoles DFT calculations

Phenyl-extended resorcin[4]arene opens up a new avenue for highly efficient iodine adsorption

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Science China chemistry 2025年第2期68卷 405-406页

作者： Jingyu Chen Jiong Zhou department of chemistry College of SciencesNortheastern UniversityShenyang 110819China

Macrocyclic arenes have become an important tool in supramolecular chemistry due to their special structure,easy functionalization and prominent host–guest *** design and synthesis of macrocyclic arenes with novel structures and excellent performances have been the focus of research in the field of supramolecular chemistry,including calixarenes,pillararenes,biphenarenes,and hybridarenes[1].These macrocyclic arenes have demonstrated significant potential and value in diverse research fields,such as crystal engineering,adsorption and separation,sensing and detection,as well as drug delivery[2].

关键词： properties adsorption iodine

Aggregation of thermally activated delayed fluorescence molecules to boost solid electrochemiluminescence efficiency for biosensing of protein-specific glycoforms

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Science China chemistry 2025年

作者： Chao Wang Zhiwei Tang Yiran Li Mengjiao Li Haijiao Xie Huangxian Ju State Key Laboratory of analytical chemistry for Life Science School of Chemistry and Chemical Engineering Nanjing University Hangzhou Yanqu Information Technology Co. Ltd.

Low quantum yield and insufficient exciton utilization of nanoemitters are great obstacles to achieving their practical electrochemiluminescence(ECL) applications. Here an aggregation strategy of thermally activated delayed fluorescence molecules was designed to reduce the energy gap between the lowest excited singlet and triplet states, and accelerate the reverse intersystem crossing of triplet excitons to the excited singlet state, which increased the exciton utilization, leading to longer delayed fluorescence lifetime and greatly boosted the quantum yield up to 87.5%, using a previously reported DMAC-TRZ as a *** aggregation could be conveniently performed by increasing the water content in the tetrahydrofuran solution of DMACTRZ. Benefiting from the high quantum yield, the solid ECL efficiency was broken through to 62.9%, much higher than the limit of 25%, and a sensitive ECL imaging method was thus proposed for simultaneous high-throughput detection of mucin1-specific sialic acid and fucose on cells by combining a ***-aided cleavage recycling to obtain the detection samples, and a DNA array to capture the detection samples and then recognize the ECL probes. This method showed good reliability and could be expanded to detect the glycans on different proteins by altering the protein aptamer sequence. This work charts a fresh course for exploiting highly efficient ECL emitters and extends their applications in ECL bioanalysis.

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Knotting ligands to control metal coordination geometry

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Science China chemistry 2025年第2期68卷 403-404页

作者： Fabien B.L.Cougnon department of chemistry and Nanoscience Centre University of JyväskyläJyväskyläFinland

Zinc is a metal of particular importance for life[1].It is the most abundant transition metal in biological systems after iron and contributes both structural and catalytic roles to many cellular *** properties of Zn^(Ⅱ),unlike those of any other first-row transition metal ions,explain its biological *** to its filled d-shell orbitals,Zn^(Ⅱ) is redox-stable,has a ligand-field energy stabilization of zero and,consequently,no typical coordination number and *** metalloproteins exploit these features to carry a broad range of chemical reactions in mild *** metalloenzymes,unsaturated ZnII centres often act as redox-stable Lewis *** protein backbone provides a highly preorganized environment around the metal centre and accompanies the changes in coordination geometry occurring as substrate transformation proceeds,thereby modulating the metal reactivity.

关键词： coordination geometry centre